技术领域technical field
本发明涉及可充电蓄电池、金属空气蓄电池、用于此类蓄电池的锌电极以及尤其可充电锌空气蓄电池。The invention relates to rechargeable batteries, metal-air batteries, zinc electrodes for such batteries and especially rechargeable zinc-air batteries.
背景技术Background technique
可充电锌空气蓄电池因其与Li离子蓄电池相当的能量密度(超过铅酸蓄电池的至少3到6倍)及其每kWh的低成本(与铅酸蓄电池相当或比铅酸蓄电池更便宜并且比Li离子蓄电池便宜5到10倍)而著名。Rechargeable zinc-air batteries due to their comparable energy density to Li-ion batteries (at least 3 to 6 times more than lead-acid batteries) and their low cost per kWh (equal to or cheaper than lead-acid batteries and cheaper than Li-ion batteries) Ion batteries are 5 to 10 times cheaper) and are famous.
这些蓄电池如果能提供足够的使用寿命将极其有利于许多应用，包含电动车辆和稳定电力存储装置。然而到目前为止，还尚未为这种类型的蓄电池提供适合应用的特点。These batteries, if they can provide sufficient service life, will be extremely beneficial for many applications, including electric vehicles and stable power storage devices. To date, however, no application-appropriate features have been provided for this type of accumulator.
例如，考虑到这些蓄电池的低成本，我们估计对于电动滑板车的最低要求将类似于：至少70Wh/kg能量密度；15W/kg功率密度以及能循环200次的6个月使用寿命。For example, given the low cost of these batteries, we estimate that the minimum requirements for electric scooters will be similar to: at least 70Wh/kg energy density; 15W/kg power density and a 6-month service life capable of 200 cycles.
发明内容Contents of the invention
具体问题Specific issues
众所周知，如果电解质不能在锌电极或充电电极室循环，那么离子的浓度就不会在整个Zn电极高度上均匀分布--尤其是锌酸盐和OH离子，并且会发生许多问题：树突会形成得更快、锌会在充电电极室中沉淀、碳化会损坏空气电极、形状改变损坏电池等，而锌酸盐离子老化也会发生。在这种情况下，循环超过10次都难以实现。It is well known that if the electrolyte is not circulated in the zinc electrode or charging electrode compartment, then the concentration of ions will not be uniformly distributed over the entire height of the Zn electrode - especially zincate and OH ions, and many problems will occur: dendrites will form faster, zinc can precipitate in the charging electrode chamber, carbonization can damage the air electrode, shape change can damage the battery, etc., and zincate ion aging can also occur. In this case, looping more than 10 times is difficult to achieve.
本发明意在排除现有技术的这些问题。The present invention intends to obviate these problems of the prior art.
众所周知，电解质循环正改善锌空气电池的循环能力。然而，以传统的方式，电解质循环是通过外部泵的方式进行的。It is well known that electrolyte cycling is improving the cycleability of Zn-air batteries. Traditionally, however, electrolyte circulation is done by means of an external pump.
发明人成功使气动提升泵(见https://en.wikipedia.org/wiki/Airlift_pump)的熟知技术相关联到锌空气电池，使得所述锌空气电池能够在充电过程中享有电解质循环而不需要外部泵送设备。The inventors succeeded in correlating the well-known technology of an airlift pump (see https://en.wikipedia.org/wiki/Airlift_pump) to a zinc-air battery, enabling said zinc-air battery to enjoy electrolyte circulation during charging without the need for External pumping equipment.
在气动提升泵中，空气被注入到输送液体的上升管的下部部分。借助于浮力，密度比液体密度更低的空气能快速地上升。在流体压力下，液体在上升的气流中被吸收，并在与空气相同的方向上移动。由于两相流的物理性质，使得可能计算流体的体积流量。这种类型的泵是极可靠的。In an air lift pump, air is injected into the lower portion of the riser pipe that conveys the liquid. Air, which is less dense than liquid, can rise rapidly due to buoyancy. Under fluid pressure, liquid is absorbed in an updraft and moves in the same direction as air. Due to the physical properties of two-phase flow, it is possible to calculate the volume flow of the fluid. This type of pump is extremely reliable.
这是所属领域的技术人员所熟知的变型，被称为“盖瑟泵(geyser pump)”，这种泵具有更大的吸力且需要更少的空气。This is a variant known to those skilled in the art, known as a "geyser pump", which has greater suction and requires less air.
本发明人观察到气动提升泵及其变型盖瑟泵都可以在锌空气电池充电过程中用于锌空气电池，以使用释放的氧气来泵送碱性电解质。相较于传统气动提升泵的操作，在本发明中，空气经由在充电过程中OH离子的电解氧化被从阳极极化条件下的电极释放的氧气取代，所述电极在整个本专利申请中被称为充电电极，并且气动提升泵所输送的液体是电池的碱性电解质。The inventors have observed that both pneumatic lift pumps and their variants, Gaiser pumps, can be used in zinc-air batteries to use released oxygen to pump alkaline electrolyte during zinc-air battery charging. In contrast to the operation of conventional pneumatic lift pumps, in the present invention the air is replaced by oxygen released from the electrodes in anodically polarized conditions, which are referred to throughout this patent application, via the electrolytic oxidation of OH ions during charging. is called the charge electrode, and the fluid delivered by the air lift pump is the battery's alkaline electrolyte.
结果result
因此，在本发明中，通过充电电极上的氧气释放保证的气动提升泵使电解质循环，从而得到非常简单、可靠且便宜的方法来防止形状改变和树突生长。Thus, in the present invention, the electrolyte is circulated by a pneumatic lift pump guaranteed by oxygen release on the charging electrode, resulting in a very simple, reliable and inexpensive method to prevent shape change and dendrite growth.
因此，本发明涉及一种供碱性电解质二次蓄电池使用的锌空气二次电池，包括Therefore, the present invention relates to a zinc-air secondary battery for alkaline electrolyte secondary batteries, comprising
-锌电极；- Zinc electrodes;
-空气电极；- air electrodes;
-用于对锌电极充电的充电电极，所述充电电极面向锌电极的至少一面，并且- a charging electrode for charging the zinc electrode, said charging electrode facing at least one side of the zinc electrode, and
所述电池包括与充电电极的至少一侧接触的一层碱性液体电解质，The battery includes a layer of alkaline liquid electrolyte in contact with at least one side of the charging electrode,
所述电池进一步包括上升管，所述上升管在开始充电时至少部分地用电解质填充，the battery further includes a riser at least partially filled with electrolyte when charging is initiated,
所述上升管包括：在其最底部的至少一个进气口，用于接收从充电释放的并最终与电解质混合的氧气；以及位于高于进气口的混合物出口，在充电过程中氧气和电解质自所述混合物出口流出，The riser includes: at least one gas inlet at its lowermost portion for receiving oxygen released from charging and ultimately mixed with the electrolyte; and a mixture outlet located above the gas inlet for oxygen and electrolyte during charging flows out from the outlet of the mixture,
所述上升管界定在所述锌电极的充电过程中仅通过从充电电极释放的氧气启动的气动提升泵，said riser defines a pneumatic lift pump activated only by oxygen released from the charging electrode during charging of said zinc electrode,
所述电池有利地包括气体收集器，所述气体收集器收集最终与电解质混合的所述释放的氧气并且最终借助于空气供应线将所述氧气传送到所述进气口。Said cell advantageously comprises a gas collector which collects said released oxygen which eventually mixes with the electrolyte and which finally conveys said oxygen to said gas inlet by means of an air supply line.
通过使用氧气释放在充电电极(辅助电极或双功能空气电极)上的起泡保证此气动提升系统在充电电极室中。氧气泡被引导通过具有有限的横截面的上升管，在所述上升管中氧气泡与电解质液体混合；并且这些氧气泡通过阿基米德定律将电解质从上升管的底部推移到应在更高水平处的上升管的输出端。如上所述，此类泵原理是熟知的“气动提升泵”及其变型“盖瑟泵”，并且在例如(http://www.uwex.edu/uwmril/pdf/RuralEnergyIssues/aquaculture/90_Air_Lift_Theory.pdf)中进行了描述。在例如JacobRiglin的荣誉论文“具有由切向流体注入引起的涡流的气动提升泵的性能特征(Performance Characteristics of Airlift Pumps with Vortex Induced byTangential Fluid Injection)”(2011年)中还可以找到一些其它变型。然而，据发明人所知，本发明是第一次尝试和描述如何将气动提升泵原理应用到电化学电池，特别是为了在没有气泡的蓄电池室中循环电解质，例如在锌电极室(包括空气电极、保证锌电极和充电电极电绝缘的分隔件，以及介于其间的电解质)中循环电解质。这种解决方案实施起来非常简单，而且有成本效益，因为它不需要任何外部泵。据发明人所知，这也是第一次描述针对其每个电池分配一个单独的泵的锌空气蓄电池。This pneumatic lift system is secured in the charge electrode chamber by bubbling with oxygen release over the charge electrode (auxiliary electrode or bifunctional air electrode). Oxygen bubbles are directed through a riser of finite cross-section where they mix with the electrolyte liquid; and these oxygen bubbles push the electrolyte from the bottom of the riser to a higher level at the output end of the riser tube. As mentioned above, such pump principles are the well-known "Air Lift Pump" and its variant "Gaiser Pump", and are described, for example, in (http://www.uwex.edu/uwmril/pdf/RuralEnergyIssues/aquaculture/90_Air_Lift_Theory.pdf ) are described. Some other variants can also be found in eg Jacob Riglin's honors thesis "Performance Characteristics of Airlift Pumps with Vortex Induced by Tangential Fluid Injection" (2011). However, to the best of the inventor's knowledge, the present invention is the first attempt and description of how the principle of a pneumatic lift pump can be applied to electrochemical cells, in particular for the circulation of electrolyte in accumulator compartments free of gas bubbles, such as in zinc electrode compartments (comprising air Electrolyte, the separator to ensure the electrical insulation of the zinc electrode and the charging electrode, and the electrolyte in between) circulate the electrolyte. This solution is very simple to implement and cost-effective as it does not require any external pumps. To the inventors' knowledge, this is also the first time a zinc-air battery has been described that assigns a separate pump to each of its cells.
有利的是，本发明涉及上文所定义的电池，其中所述气动提升泵的混合物输出端最少比所述进气口高20mm，由此提供足够的电解质输送能力和输送效率。Advantageously, the invention relates to a battery as defined above, wherein the mixture output of said pneumatic lift pump is at least 20mm higher than said inlet, thereby providing sufficient electrolyte delivery capacity and delivery efficiency.
有利的是，本发明涉及上文所定义的电池，其中上升管具有表面小于或等于15mm2的横截面，且有利地具有等于或大于2mm2的横截面。Advantageously, the invention relates to a battery as defined above, wherein the riser has a cross-section with a surface less than or equal to 15 mm2 , and advantageously has a cross-section equal to or greater than 2 mm2 .
应注意，上升管的横截面不应太大，否则没有气动提升效果。优选地，所述上升管的内径为从1mm和4mm，优选地2mm的直径，或有利的是，上升管具有1mm2到14mm2之间的横截面。It should be noted that the cross-section of the riser should not be too large, otherwise there will be no aerodynamic lifting effect. Preferably, the inner diameter of the riser is from 1 mm and 4 mm, preferably a diameter of 2 mm, or advantageously the riser has a cross-section between 1 mm2 and 14 mm2 .
有利的是，本发明涉及上文所定义的电池，其中在充电过程中上升管基本上是竖直的。Advantageously, the invention relates to a battery as defined above, wherein the riser tube is substantially vertical during charging.
有利的是，本发明涉及上文所定义的电池，其中上升管定位高于锌电极的顶部。Advantageously, the invention relates to a battery as defined above, wherein the riser is positioned higher than the top of the zinc electrode.
有利的是，本发明涉及上文所定义的电池，其中所述电池还包含膨胀储槽，接收充电过程中的气动提升泵的输出流量、电解质和充电过程中释放的氧气的混合物；所述膨胀储槽包括至少排气口(用于氧气排出)。Advantageously, the invention relates to a battery as defined above, wherein said battery further comprises an expansion reservoir receiving a mixture of the output flow of the pneumatic lift pump during charging, electrolyte and oxygen released during charging; said expansion The storage tank includes at least a vent (for oxygen venting).
有利的是，本发明涉及上文所定义的电池，其中所述膨胀储槽连通到锌空气电池的底部，由此允许电解质在充电过程中回流及循环。Advantageously, the present invention relates to a battery as defined above, wherein said expansion reservoir communicates to the bottom of the zinc-air battery, thereby allowing backflow and circulation of the electrolyte during charging.
有利的是，本发明涉及上文所定义的电池，其中膨胀储槽连接到回流管，所述回流管连接到电池底部的电解质回流口。Advantageously, the invention relates to a battery as defined above, wherein the expansion reservoir is connected to a return conduit connected to an electrolyte return opening at the bottom of the battery.
有利的是，本发明涉及上文所定义的电池，其中在充电开始时膨胀储槽中电解质的水平至少比所述空气输入端高最少20mm，由此压头足以开始并维持电解质循环。Advantageously, the invention relates to a battery as defined above, wherein the level of electrolyte in the expansion tank is at least 20 mm above said air input at the start of charging, whereby the head pressure is sufficient to initiate and maintain electrolyte circulation.
有利的是，本发明涉及上文所定义的电池，其中气动提升泵、膨胀储槽和回流管全部共用同一壳体，由此简化设计和互连件数量。Advantageously, the invention relates to a battery as defined above, wherein the air lift pump, expansion tank and return pipe all share the same housing, thereby simplifying the design and the number of interconnections.
贯穿本发明，通过“锌电极室”来指包括锌电极以及在所述锌电极与保证所述锌电极和充电电极电绝缘的分隔件之间的电解质的空间。Throughout the present invention, by "zinc electrode compartment" is meant the space comprising the zinc electrode and the electrolyte between said zinc electrode and the separator ensuring electrical insulation of said zinc electrode and charging electrode.
类似地，贯穿本发明，通过“充电电极室”来指包括充电电极以及在所述充电电极与保证所述锌电极和所述充电电极电绝缘的分隔件之间的电解质的空间。Similarly, throughout the present invention, by "charging electrode compartment" is meant the space comprising the charging electrode and the electrolyte between said charging electrode and the separator ensuring electrical insulation of said zinc electrode and said charging electrode.
在充电开始时，许多氧气泡在充电电极的表面上快速释放并且与充电电极室的电解质混合。氧气泡取代了被推移到电极室之外的一些体积的电解质。因此，适宜地，电池的气动提升泵的输出端连接到膨胀储槽和排气口以允许氧气逸出电池，所述膨胀储槽足够大以承受保持不仅电解质而且电池内部氧气体积所需的体积的增加。At the beginning of charging, many oxygen bubbles are rapidly released on the surface of the charging electrode and mix with the electrolyte of the charging electrode chamber. Oxygen bubbles displace some of the volume of electrolyte that is pushed out of the electrode compartment. So suitably the output of the cell's air lift pump is connected to an expansion reservoir large enough to take up the volume required to hold not only the electrolyte but also the oxygen volume inside the cell to allow oxygen to escape the cell and a vent to allow oxygen to escape the cell increase.
最后，膨胀储槽有利地连接到电池底部，使得电解质可以循环并回流到电池。Finally, an expansion reservoir is advantageously connected to the bottom of the battery so that the electrolyte can circulate and flow back into the battery.
此外，在本发明中，考虑到氧气释放速率直接关联到充电电流，有利地调整上升管的所述横截面以控制电解质的循环速率。Furthermore, in the present invention, said cross-section of the riser is advantageously adjusted to control the circulation rate of the electrolyte, considering that the oxygen release rate is directly related to the charging current.
本发明还涉及包括根据以上定义的至少一个电池的锌空气蓄电池系统。The invention also relates to a zinc-air battery system comprising at least one battery according to the above definition.
有利的是，本发明涉及以上锌空气蓄电池，其中多个电池共用共同的电解质膨胀储槽。Advantageously, the present invention relates to the above zinc-air battery, wherein a plurality of cells share a common electrolyte expansion reservoir.
本发明涉及一种包括如上文所定义的锌空气蓄电池的车辆。The invention relates to a vehicle comprising a zinc-air battery as defined above.
[共混][blend]
众所周知，在充电过程中，当电解质流过阳极和阴极室同时一些电流在电池中流动时，在阳极和阴极附近电解质的pH值发生改变。在对锌空气电池充电的情况下，当流过锌电极室时pH值将增大，并且当流过充电对电极室时pH值将减小。在电池单元包含锌电极的情况下，还众所周知，强碱性电解质中ZnO的溶出取决于1(ZnO的)到10(KOH)的比率下的KOH浓度，然而，在更强KOH溶液中，溶出率增加。在充电过程中，这可能导致在充电电极附近ZnO沉淀，最终导致在Zn电极的有效质量在进一步循环过程中变得耗尽时锌酸盐离子老化。因此，根据本发明的优选方式，为了避免当电解质的pH值减小时Zn在充电电极室中沉淀，应使电池的电解质循环组织为使得分流共同电解质流以供应锌室和充电室，并且对来自锌电极室和充电电极室的电解质输出进行分组和共混，之后再在电池底部作为共同电解质流引入，由此平均锌室和充电室中电解质的pH值。It is well known that during charging the pH of the electrolyte changes in the vicinity of the anode and cathode as the electrolyte flows through the anode and cathode compartments while some current flows in the battery. In the case of charging a zinc-air battery, the pH will increase when flowing through the zinc electrode chamber and decrease when flowing through the charging counter electrode chamber. In the case of cells containing zinc electrodes, it is also known that the dissolution of ZnO in strongly alkaline electrolytes depends on the KOH concentration at a ratio of 1 (of ZnO) to 10 (of KOH), however, in stronger KOH solutions, the dissolution rate increase. During charging, this can lead to precipitation of ZnO near the charging electrode, eventually leading to aging of zincate ions when the effective mass of the Zn electrode becomes depleted during further cycling. Therefore, according to a preferred mode of the invention, in order to avoid precipitation of Zn in the charging electrode compartment when the pH value of the electrolyte decreases, the electrolyte circulation of the battery should be organized in such a way that the common electrolyte flow is split to supply the zinc compartment and the charging compartment, and the The electrolyte outputs from the zinc and charge electrode compartments are grouped and blended before being introduced at the bottom of the cell as a common electrolyte flow, thereby averaging the pH of the electrolyte in the zinc and charge compartments.
还观察到，使用在此提出的电解质循环方法不可能产生过饱和锌酸盐电解质。不稳定的过饱和锌酸盐电解质随时间推移会变得与电池任何位置的所得ZnO沉淀饱和，同样使锌酸盐离子老化。It was also observed that it was not possible to produce a supersaturated zincate electrolyte using the electrolyte cycling method proposed here. An unstable supersaturated zincate electrolyte becomes saturated with the resulting ZnO precipitates anywhere in the cell over time, similarly aging the zincate ions.
附图说明Description of drawings
图1figure 1
[图1]是第US 2007/0166171号申请中所公开的气动提升泵的示意性图示。所述气动提升泵通过压缩空气功能，通过夹带气体使流体上升以减小其密度。1.空气供应。2.液体供应。3.进气口。4.空气供应线。5.空气口。6.出气口。7.流体入口。8.上升管。9.空气液体混合物。10.泵出口。L：液体，通常是废水。LL：液位。V：容器。G：砾石或固体。[ Fig. 1 ] is a schematic illustration of an air lift pump disclosed in Application No. US 2007/0166171. The air lift pump functions by compressing air, causing the fluid to rise by entraining gas to reduce its density. 1. Air supply. 2. Liquid supply. 3. Air intake. 4. Air supply line. 5. Air port. 6. Air outlet. 7. Fluid inlet. 8. Riser tube. 9. Air-liquid mixture. 10. Pump outlet. L: Liquid, usually waste water. LL: liquid level. V: container. G: Gravel or solid.
图2figure 2
[图2]是根据本发明的电极在充电过程中当气动提升泵启动时的示意性图示。1.具有15Ah、150mm高、120mm宽、10mm厚的电化学电池(包含空气电极、充电电极和锌电极，竖直地安装，彼此平行)。电解质是6M KOH。2.与电解质混合的氧气泡。3.高10mm的气体收集器。4.进气口。5.上升管，内部横截面直径2mm的PVC管。6.空气液体混合物输出流。7.排气口，直径2mm的孔。8.膨胀储槽，高＝70mm、宽＝40mm、厚＝12mm，储槽底部位于电化学电池顶部以上50mm。在开始充电时储槽上升直至大致10mm的水平。9.回流管，横截面内部直径4mm的PVC管。10.电解质回流口。[ Fig. 2 ] is a schematic illustration of an electrode according to the present invention when an air lift pump is activated during charging. 1. An electrochemical cell of 15Ah, 150mm high, 120mm wide, 10mm thick (comprising air electrode, charge electrode and zinc electrode, mounted vertically, parallel to each other). The electrolyte is 6M KOH. 2. Oxygen bubbles mixed with electrolytes. 3. Gas collector with a height of 10mm. 4. Air intake. 5. Riser pipe, PVC pipe with an internal cross-sectional diameter of 2 mm. 6. Air-liquid mixture output flow. 7. Exhaust port, a hole with a diameter of 2mm. 8. Expansion storage tank, height = 70mm, width = 40mm, thickness = 12mm, the bottom of the storage tank is located 50mm above the top of the electrochemical cell. The reservoir rises to a level of approximately 10mm at the start of charging. 9. Return pipe, a PVC pipe with an internal diameter of 4 mm in cross section. 10. Electrolyte return port.
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US201562157848P | 2015-05-06 | 2015-05-06 | |
| US62/157,848 | 2015-05-06 | ||
| PCT/IB2016/052594WO2016178186A1 (en) | 2015-05-06 | 2016-05-06 | Zinc-air cell with airlift pump |
| Publication Number | Publication Date |
|---|---|
| CN107836052Atrue CN107836052A (en) | 2018-03-23 |
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201680039879.8APendingCN107836052A (en) | 2015-05-06 | 2016-05-06 | Zinc-air battery with pneumatic lift pump |
| Country | Link |
|---|---|
| EP (1) | EP3292577A1 (en) |
| CN (1) | CN107836052A (en) |
| WO (4) | WO2016178186A1 (en) |
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| WO2016178187A1 (en) | 2016-11-10 |
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| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| WD01 | Invention patent application deemed withdrawn after publication | Application publication date:20180323 | |
| WD01 | Invention patent application deemed withdrawn after publication |